Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO2 Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer

Qi, Zhen; Kashi, Ajay R.; Buckley, Aya K.; Miller, John S.; Ye, Jianchao; Biener, Monika M.; Foucher, Alexandre C.; Stach, Eric A.; Ma, Sichao; Kuhl, Kendra P.; Biener, Juergen

doi:10.1021/acs.jpcc.2c03773

Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO₂ Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer

Journal Article · Tue Nov 08 23:00:00 EST 2022 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.2c03773· OSTI ID:1902016

^[1]; Kashi, Ajay R. ^[2]; Buckley, Aya K. ^[2]; Miller, John S. ^[1]; ^[1]; ^[1]; ^[3]; ^[3]; Ma, Sichao ^[2]; Kuhl, Kendra P. ^[2]; ^[1]

Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)
Twelve Benefit Corporation, Berkeley, CA (United States)
University of Pennsylvania, Philadelphia, PA (United States)

We report catalyst surface area and wetting behavior are key factors in determining the performance of gas diffusion electrode (GDE) electrolyzers for electrochemical CO₂ reduction. In this work, we report the integration of sub-1 μm thick nanoporous gold (npAu) catalyst coatings into a large-area (25 cm²) zero-gap electrolyzer. The npAu coatings were prepared by magnetron sputtering (MS) of thin AgAu alloy films on the microporous carbon layer of a gas diffusion layer (GDL) followed by Ag leaching. Compared to MS Au films of the same thickness, npAu catalyst coatings enable higher Faradaic efficiencies and improved catalyst stability for CO₂-to-CO reduction with Faradaic efficiencies of up to 88% at 100 mA/cm². For a 800 nm npAu coating, the device level energy efficiency for CO₂ to CO conversion reaches 45% (52% for CO + H₂) at 100 mA/cm² with a single pass CO₂ conversion efficiency of ~12%. Contact angle measurements reveal that npAu coatings provide a more hydrophobic electrode interface compared to MS Au coatings, suggesting that the more hydrophobic interfacial environment of npAu coatings helps mitigating electrode flooding which is associated with performance deterioration over time.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Livermore National Laboratory (LLNL), Livermore, CA (United States)

Sponsoring Organization:: USDOE National Nuclear Security Administration (NNSA); USDOE Office of Energy Efficiency and Renewable Energy (EERE); National Science Foundation (NSF)

Grant/Contract Number:: AC52-07NA27344; AC02-05CH11231

OSTI ID:: 1902016

Report Number(s):: LLNL-JRNL-834289; 1052662

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 46 Vol. 126; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO2 Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer

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Effect of Gold Catalyst Surface Morphology on Wetting Behavior and Electrochemical CO₂ Reduction Performance in a Large-Area Zero-Gap Gas Diffusion Electrolyzer